In organic electronic devices made with organic thin films, the morphology (e.g., the crystal structure) of the organic films can play a role in determining the electronic and/or optical properties of the device. In many cases, the organic molecules in the films exhibit a pronounced anisotropy, and the orientation of the organic molecules within the film can influence charge carrier mobility. For example, creating crystalline order within an organic film of an organic light emitting device can reduce series resistance, and thereby increase luminous efficiency. In organic photosensitive devices such as organic photovoltaic (OPV) devices, creating crystalline order within an organic film of the photosensitive devices can increase the short-circuit current Jsc and the open-circuit voltage Voc. For example, controlling the molecular crystalline orientation of the donor layer for example can lead to beneficial changes in the frontier energy levels, absorption coefficient, morphology, and exciton diffusion length, resulting in an increase in the PV cell's power conversion efficiency, ηp. Furthermore, because crystalline structures are morphologically more stable than amorphous structures, the resulting devices would have the potential for greater long term operational reliability. While it is clear that the crystal structure of the organic molecules in an organic thin film can be an important feature of the devices, it has been difficult to achieve the desired film crystal structure. In particular, creating a multilayer crystalline organic film structure in which a quasi-epitaxial relationship is maintained through the multiple layers of crystalline organic thin film layers, similar to the inorganic semiconductor quantum wells, has not been achieved previously. Thus, there is a need for improved methods for growing multiple layers of crystalline organic films having a desired crystal structure for use in optoelectronic devices.